Zinc Reverse Diffusion‐Induced Uniform Lithium Deposition in Composite Metal Anodes for High‐Performance Lithium Metal Pouch Batteries

ABSTRACT Lithium‐metal batteries are promising for overcoming the energy‐density limitations of conventional lithium‐ion batteries, but dendrite growth and interfacial instability hinder their practical application. Traditional static control strategies struggle to maintain lithiophilicity at the advancing deposition front during high‐areal‐capacity plating. Here, we construct a bulk‐homogeneous Li/LiZn–Li 2 O composite anode using a scalable in situ metallurgical strategy, in which one‐dimensional LiZn forms a continuous transport/support network, while nanoscale Li 2 O provides dispersed polar lithiophilic sites. Theoretical calculations show that the LiZn surface lowers the Li surface‐migration barrier to 0.25 eV, whereas Li 2 O thermodynamically anchors Li species and promotes uniform nucleation. Moreover, Zn species migrate toward the growth front during deposition, continuously replenishing lithiophilic sites and enabling dynamic interfacial regulation. The Li/LiZn–Li 2 O composite anode enables near‐theoretical dense Li deposition, with a thickness expansion rate of only 5.09 µm (mAh cm −2 ) −1 , and sustains stable cycling for over 1210 h at 6 mA cm −2 and 6 mAh cm −2 . It can be roll‐processed into an ultrathin 20 µm foil and delivers 476.6 Wh kg −1 in a 3 Ah‐level pouch cell with a high‐loading NCM811 cathode. This work offers a route to high‐performance Li‐metal anodes with dynamically adaptive interfaces.